Title: Steering CO ₂ electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon

Abstract

Electrochemical reduction of CO₂to multicarbon products is a significant challenge, especially for molecular complexes. In this work, we report CO₂reduction to multicarbon products based on a Ru(II) polypyridyl carbene complex that is immobilized on an N-doped porous carbon (RuPC/NPC) electrode. The catalyst utilizes the synergistic effects of the Ru(II) polypyridyl carbene complex and the NPC interface to steer CO₂reduction toward C2 production at low overpotentials. In 0.5 M KHCO₃/CO₂aqueous solutions, Faradaic efficiencies of 31.0 to 38.4% have been obtained for C2 production at -0.87 to -1.07 V (vs. normal hydrogen electrode) with 21.0 to 27.5% for ethanol and 7.1 to 12.5% for acetate. Syngas is also produced with adjustable H₂/CO mole ratios of 2.0 to 2.9. The RuPC/NPC electrocatalyst maintains its activity during 3-h CO₂-reduction periods.

Authors:

Liu, Yanming ^[1]; Fan, Xinfei ^[2]; Nayak, Animesh ^[3]; Wang, Ying ^[3]; Shan, Bing ^[3]; Quan, Xie ^[4]; Meyer, Thomas J.  ^[3]

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+ Show Author Affiliations

1. Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China,, Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599,
2. College of Environmental Science and Engineering, Dalian Maritime University, Dalian 116024, China
3. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599,
4. Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China,

Publication Date:

2019-12-10

Research Org.:

Univ. of North Carolina, Chapel Hill, NC (United States)

Sponsoring Org.:

USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC)

OSTI Identifier:

1577930

Alternate Identifier(s):

OSTI ID: 1802763

Grant/Contract Number:  

SC0015739; 21707016; 51708085

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 52; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 reduction; electrocatalysis; Ru(II) polypyridyl complex; porous carbon